Effect of MnO2 doped on physical, structure and optical properties of zinc silicate glasses from waste rice husk ash 1 3 4 5 6 7 8 9 10 1 2 13 14 15 16 17 18 19 20 21 22 23 24 25 2 6 45 46 47 48 49 50[.]
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6
7 Ali Jabbar Abed Al-Nidawia, Khamirul Amin Matoria,b,⇑, Azmi Zakariaa, Mohd Hafiz Mohd Zaida,b
Department of Physics, Faculty of Science, Universiti Putra Malaysia, 43400 UPM Serdang, Selangor, Malaysia
Materials Synthesis and Characterization Laboratory, Institute of Advanced Technology, Universiti Putra Malaysia, 43400 UPM Serdang, Selangor, Malaysia
10
1 2 a r t i c l e i n f o
13 Article history:
14 Received 26 January 2017
15 Received in revised form 14 February 2017
16 Accepted 15 February 2017
17 Available online xxxx
18 Keywords:
19 Rice husk
20 Manganese dioxide
21 Glass
22 Zinc silicate
23 Sintering
24 Optical properties
25
2 6
a b s t r a c t
27
In this study, an investigation was conducted to explore and synthesize silicate (SiO2) glass from
28
29 [(ZnO)55+ (WRHA)45]100-X[MnO2]X, (where X = 0, 1, 3 and 5 wt%) was prepared by conventional melt
30 quenching technique The glass samples were characterized using energy dispersive X-ray fluorescence
31 (EDXRF), X-ray diffraction (XRD), field emission scanning electron microscopy (FESEM), Fourier transform
32 infrared (FTIR) spectroscopy, and ultraviolet–visible (UV–Vis) spectroscopy The results revealed that by
33 increasing the concentration of MnO2, the color of glass samples changed from colorless to brown and the
34 density of glass increased XRD results showed that a broad halo peak which centered on the low angle
35 (2h = 30°) indicated the amorphous nature of the glass FTIR results showed basic structural units of
36 Si-O-Si in non-bridging oxygen, Si-O and Mn-O in the glass network FESEM result showed a decreasing
37 porosity with an increasing MnO2content, which was attributed to the Mn ions resort to occupy
inter-38 stitial sites inside the pores of glass Besides, the absorption intensity of glass increased and the band
39 gap value decreased with increasing the MnO2percentage In this synthesized glass system of MnO2
40 doped zinc silicate glasses using RHA as a source of silica, the MnO2affect most of the properties of
41 the glass system under investigation
42
Ó 2017 Published by Elsevier B.V This is an open access article under the CC BY-NC-ND license (http://
43 creativecommons.org/licenses/by-nc-nd/4.0/)
44 45
46 Introduction
47 Rice husk (RH) is one of the agricultural waste materials that
48 received high attention because of its high amount of silica
con-49 tent Generally, in Malaysia for each 1000 kg of paddy milled,
50 220 kg (22%) of rice husk will be produced The subsequent
burn-51 ing of the rice husk will generate about 55 kg (25%) of rice husk
52 ash (RHA)[1] RHA have many good properties such as high
poros-53 ity, high external surface area, lightweight, and high in silica
con-54 tent inform of amorphous materials (87–97%) and a few metallic
55 impurities[2,3] Rice husk is an agricultural waste material that
56 is renewable and has low bulk density Unfortunately, this waste
57 is left to rot slowly in the field or burnt in an open space Many
sug-58 gest that recycling of the waste is the best way compared to these
59 unsafe disposals procedure several advantages such as resources
60 and energy saving, reduces incineration and helps in protecting
61
the environment[4–6] Nowadays, various researchers have done
62
many works toward utilizations of the waste materials in various
63
industries and as an additive in manufacturing some products
64 [7] Specifically, RHA had been used for development of advanced
65
materials and utilization in many areas Different processing
tech-66
niques and treatments were employed and effect of various
param-67
eters were studied [8,9] Currently, a considerable amount of
68
literature has been published on the use of glass in a wide range
69
of applications in many industries such as automotive, aerospace,
70
electrical, electronic and telecommunication Therefore, intensive
71
research has been carried out in order to improve the properties
72
of the glass, reduce the cost of the material and at the same lower
73
the fabrication cost These motivate researchers to developed new
74
fabrication techniques and utilization of waste materials for better
75
wealth and clean environment Therefore, the aforementioned
76
objectives could be achieved using RH, which is available and
77
abundant and will definitely lower the cost of final products
78
In 2011, Ruangtaweep and coworkers fabricate a glass using
79
55SiO2from RHA with the different formula of 20 Na2O, 13 B2O3,
80
6.3 CaO, 1.0 Al2O3, 0.2 Sb2O3, and 4.5 BaO by melt quenching
81
method at 1100°C The results of the study indicated that the
den-82
sity of glass derived from RHA is larger than pure SiO2 The results http://dx.doi.org/10.1016/j.rinp.2017.02.020
2211-3797/Ó 2017 Published by Elsevier B.V.
This is an open access article under the CC BY-NC-ND license ( http://creativecommons.org/licenses/by-nc-nd/4.0/ ).
⇑ Corresponding author at: Department of Physics, Faculty of Science, Universiti
Putra Malaysia, 43400 UPM Serdang, Selangor, Malaysia.
E-mail addresses: alnedaweali@yahoo.com (A.J.A Al-Nidawi), khamirul@upm.
edu.my (K.A Matori), azmizak@upm.edu.my (A Zakaria), mhmzaid@gmail.com (M.
H.M Zaid).
Contents lists available atScienceDirect
Results in Physics
j o u r n a l h o m e p a g e : w w w j o u r n a l s e l s e v i e r c o m / r e s u l t s - i n - p h y s i c s
Please cite this article in press as: Al-Nidawi AJA et al Effect of MnO doped on physical, structure and optical properties of zinc silicate glasses from waste
Trang 283 further confirmed that the RHA could be used for color glass
pro-84 duction[10] Insiripong et al (2013) synthesized a glass material
85 using high purity Na2CO3, B2O3, Al2O3, CaO, BaO, Sb2O3, and SiO2
86 from RHA In this research, the RH was sintered at 1000°C and
87 use as a SiO2source for glass production The physical properties
88
and the absorption peak were examined after doping RHA with
dif-89
ferent concentration of MnO2from 0.0 to 1.0 mol% The findings
90
revealed that the color of the glass changes from colorless to brown
91
by a gradual increase of MnO2 concentration Both density and
92
reflective index were also increased with the increasing of MnO2
93
concentration, largely, due to the altered atomic volume and an
94
atomic mass of the glass[11]
95
The focus of this study is to improve the properties of glasses
96
using white rice husk ash (WRHA) as a source of SiO2by preparing
97
zinc silicate glasses doped with MnO2using conventional melt and
98
quenching method The physical, structure and optical properties
99
of MnO2 doped zinc silicate glasses have been characterized to
100
study the effect of various concentrations of MnO2 on the glass
101
samples
102
Experimental work
103
Preparation of white rice husk ash
104
The rice husk used in this research was obtained from Tanjung
105
Karang, Selangor, Malaysia To prepare the white RHA, the husks
106
was thoroughly washed with tap water up to three times to
107
remove adhering soil and dust Later the husk was rinsed with
dis-108
tilled water to remove dirt and aqueous soluble substances by
109
repeated stirring and decanting until the aqueous wash turned
110
clear The cleaned RH was then dried in an oven at 100°C for
111
24 h The RH samples were later transferred into an electric furnace
112
for a double stage heating process at 500°C for 1 h and 900 °C for
113
3 h The burnt samples could cool to room temperature as seen in
114
the temperature cycle curve inFig 1
115
Preparation of ZnO-WRHA glasses
116
The pure powder of ZnO was mixed with WRHA The
117
mixture was doped with MnO2 in different ratio (X = 0, 1, 3,
118
and 5 wt%) ascribed to the empirical formula [(ZnO)55+
119
(WRHA)45]100-X[MnO2]X Dried milling process was carried out on
120
the mixture for 20 h to get homogenous powder Each batch of
121
the samples was placed in an alumina crucible and melted in an
122
electrical furnace at 1400°C for 2 h The melts samples were then
900 °C
500 °C
3 hours
1 hour
Room temperature
Time (Hours) Fig 1 Heating circle for burning rice husk.
Table 1 Chemical composition of WRHA.
Components Percentage by weight
p o s i t i o n ( 2 T h e t a )
S ( 2 0 0 )
S ( 1 0 1 )
S ( 1 1 1 )
S ( 1 0 2 )
S ( 2 0 2 )
S ( 2 1 2 )
S ( 3 0 1 )
S ( 3 0 2 )
Trang 3123 quenched in water to get glass frits After that, un-doped and
124 doped samples were crushed and ground to 63lm size powder
125 and compacted using a hydraulic press to get pellets of 13 mm
126 diameter and2 mm thick All the samples were stored in plastic
127 bags for further experimental investigations The density of the
128 glass samples was measured with electronic densitometer
MD-129 300S carried out at room temperature Other properties
investi-130 gated and analyzed using XRD, FTIR, FESEM, and UV–Visible
131 spectroscopy
132
Results and discussion
133
Characterization of WRHA
134
The chemical composition of WRHA sintered at 900°C for 3 h
135
was analyzed by (EDXRF) and the results are shown in Table 1
136
As seen in the table, the major constituent of WRHA is SiO2 at
137
94.34%, while other oxides (P2O5, K2O, CaO, Na2O, MgO, SO3,
138
Fe2O3,MnO, and ZnO) account for the remaining percentage This
Fig 3 FTIR result for WRHA.
2.85 2.9 2.95 3 3.05 3.1 3.15 3.2 3.25 3.3
3)
MnO2(wt.%)
(2.88)
(3.25)
Fig 4 Density of MnO 2 doped ZnO-WRHA glasses.
Please cite this article in press as: Al-Nidawi AJA et al Effect of MnO doped on physical, structure and optical properties of zinc silicate glasses from waste
Trang 4139 result is consistent with previous studies which found the silica
140 contents in WRHA to be 94.3% and 92–97%[12,13]
141 The XRD analysis was done with PANalytical (Philips) X’ Pert
142 Pro PW3050/60 The XRD patterns of the sample are presented in
143 Fig 2 The pattern exhibits a sharp Bragg’s peaks at a low angle
144 region, which is apparent to the crystalline phase of silica after
145 RHA, have been heated to 900°C The figure also indicated different
146 peaks of crystalline components in the phase of cristobalite crystal
147 (SiO2) with the most intense peak at 22.049° and obviously, the
148 weak peaks at 28.451°, 31.543°, and 36.202°, respectively
149 The major chemical functional groups present in WRHA are
150 identified by the FTIR and the spectra are shows inFig 3 Looking
151 at the figure, the band at 3037.81 cm1was due to OH groups and
152 absorbed water [14] The predominant absorbance peak at
153 1606.66 cm1belonged to H-O-H bending vibration Besides, the
154 band at 1054.85 cm1 is assigned to the (Si-O-Si) asymmetry
155 stretching vibrations[15] Finally, there are two sharp bands at
156 783.22 and 441.85 cm1assigned to Si-O-Si symmetric stretching
157 and bending vibration respectively The results of the FTIR
con-158 firmed the presence of SiO2 in WRHA, which agreed well with
159 the XRD analysis
160 Properties of MnO2doped ZnO-WRHA glasses
161 Fig 4shows the density of ZnO-WRHA glasses at different
con-162 centration of MnO2(0, 1, 3 and 5 wt%) The results in the figure
163 showed that the density of the ZnO-WRHA glass increased from
164 2.885 to 3.253 g/cm3with increased of MnO2at 0, 1, 3 and 5 wt
165 % This increased in density is related to the atomic mass of Mn
166 (54.938 a.m.u) which is heavier when compared with other
ele-167 ments presence in the WRHA sample such as Si (28.086 a.m.u),
168 Na (22.989 a.m.u), and Ca (40.078 a.m.u)[16] In addition, other
169 researchers related this development to the figuration of the new
170 linkages inside the glass sample[17]
171 X-ray diffraction (XRD) patterns for all ZnO-WRHA glasses
sys-172 tem at various percentages of MnO2is shown inFig 5 From the
173 spectra, there is no strong sharp peak but one a broad halo peak
174 in the pattern of the un-doped and MnO2doped ZnO-WRHA based
175
glass samples The broad diffuse is around low angle 30° in entire
176
glasses samples, which reflected glass or amorphous nature of the
177
samples In addition, the glass under investigation has a long-range
178
structural disorder
179
The structure of all the glasses samples was determined with
180
the aid of FESEM as shown inFig 6 The results revealed the
pres-181
ence of fine pores on the ZnO-WRHA glass in an undoped sample
182
Despite the absence of a particular form of grain after doped, but in
183
general, the surface morphology shows a decrease in the number
184
of pores with increasing the percentage of MnO2 As seen in the
185
microstructural image of the samples prepared at different
per-186
centage of MnO2, the Mn resort to occupy interstitial sites within
187
the structure of the glass The lattice constant of glass increased
188
slightly with increasing concentration of MnO2, which leads to
189
increase of the degree of agglomeration that can be observed by
190
comparing the surface morphology inFig 6(a-d)[18]
191
The spectrums from FTIR results are shown inFig 7and it was
192
analyzed and compared with the relative information in the
liter-193
ature[19,20] The effective range of the spectrum observed from
194
400 to 1250 cm1, with the prominent band at 902.4 cm1ascribed
195
to Si-O-Si stretching in non-bridging oxygen[21] This peak
indi-196
cates the presence of SiO4in the sample The result from FTIR is
197
in good agreement with the result of XRD spectroscopy, which
198
revealed an amorphous phase for the entire glass samples On
199
the other hand, the peak at 1200–4000 cm1was clearly due to
200
the presence of water, hydroxyl, Si-OH or similar groups [22]
201
Therefore, the bands at 1555.85 could indicate Si-O or Mn-O, which
202
gives rise to an IR peak The peak at 3032.79 could be attributed
203
present H-bonding of H2O Furthermore, Zhang and Jahanshahi
204
suggests that this band might ascribe to absorb moisture from
205
the air[23]
206
The analysis of the optical absorption spectra is useful to locate
207
the width to the band gap in order to identify the substance from
208
the spectrum emitted or absorbance light in the material[24] The
209
optical absorbance of the MnO2 doped zinc silicate glasses is
210
shown inFig 8 As shown from the absorption curve, there is no
211
big sharp absorption edge, which dictates the presence glass phase
212
From the absorption curve, it can be observed that with increase of
0
1 0 0 0
2 0 0 0
3 0 0 0
4 0 0 0
5 0 0 0
P osition (2 T heta)
5 w t %
3 w t %
1 w t %
u n d o p e d
Fig 5 XRD pattern of MnO 2 doped ZnO-WRHA glasses.
Trang 5213 MnO2 concentration, the absorption intensity increased and
214 the intensive absorption, which can be seen in the range of
215 250–350 nm[25]
216 The optical band gap in the amorphous system is closely related
217 to the energy gap between the valence band and conduction band
218 In the amorphous system, the condition band affects by the new
219 glass formation anions The relation between absorption
coeffi-220
cient and extinction coefficient (K) in the equation below
determi-221
nes the experimental value of optical band gap:
222
225
From the plot of the extinction coefficient versus hv, the
exper-226
imental value for the optical band gap was extrapolating from the
227
linear region of the extinction coefficient (K) to zero After
Fig 6 FESEM image of MnO 2 doped ZnO-WRHA glasses, (a) undoped (b) 1 wt% (c) 3 wt% and (d) 5 wt%.
Please cite this article in press as: Al-Nidawi AJA et al Effect of MnO doped on physical, structure and optical properties of zinc silicate glasses from waste
Trang 6228 compiled all the obtained Egvalues inTable 2, a good agreement
229 between the Egin the differential curve with the value in n = 3/2
230 can be observed Hence, the obtained experimental value of the
231 optical band gap arises in the glass system by direct forbidden
232 transitions The optical band gap value decreased from 4.70 to
233 4.21 with increasing the MnO2 percentage as can be seen in the
234 Fig 9 According to the literature review, with an increase in
235
MnO2in the glass network might lead to the breakdown of SiO4
236
network consequence to product non-bridging oxygen, whereby
237
the electrons were loosely bonded to NBO’s than BO’s[26]
238
Conclusions
239
A series of ZnO-WRHA glasses doped MnO2were prepared by
240
melt quenching technique with aim of studying the effect of
vari-241
ous concentration of MnO2on the physical, structure and optical
242
properties of the glass samples Upon density measurement by
243
Archimedes’ principle, the density increased from 2.885 to
244
3.253 g/cm3with increased in the percentage of MnO2from 0, 1,
245
3 and 5 wt% The XRD confirmed the formation of the amorphous
246
glassy phase in the samples The results from FTIR agreed with
247
the XRD pattern with a band at 902.4 cm1, which was attributed
248
to Si-O-Si stretching in non-bridging oxygen’s The FESEM images
249
shows decrease trend in the number of pores with increasing
per-250
centage of MnO2and glassy phase of samples From the absorption
251
curve, it can be observed with the increasing concentration of
252
MnO2, the absorption intensity increased and intensive absorption
253
can be seen in the range from 250 to 350 nm From the results of
254
the UV–visible spectroscopy, the optical band gap value decreased
Fig 7 FTIR spectra of MnO 2 doped ZnO-WRHA glasses.
0
0.2
0.4
0.6
0.8
1
1.2
wavelength (nm)
undoped
1 wt %
3 wt %
5 wt %
Fig 8 Absorption spectra of MnO 2 doped ZnO-WRHA glasses.
Table 2
Variation of Eopt for MnO 2 doped ZnO-WRHA glasses.
n = 2 in the indirect allowed transition 4.871 ± 0.03 4.42 ± 0.03 3.93 ± 0.03 3.93 ± 0.03
n = 3 in the indirect forbidden transition 4.08 ± 0.03 4.47 ± 0.03 3.41 ± 0.03 3.29 ± 0.03
n = 1/2 in the direct allowed transition 5.16 ± 0.03 5.14 ± 0.03 5.09 ± 0.03 5.05 ± 0.03
n = 3/2 in the direct forbidden transition 4.7 ± 0.03 4.61 ± 0.03 4.42 ± 0.03 4.21 ± 0.03
Trang 7255 from 4.70 to 4.21 with increasing of MnO2percentage due to the
256 defect MnO2 in the samples and product non-bridging oxygen’s,
257 which leads to the breakdown of SiO4network
258 Acknowledgement
259 The authors gratefully acknowledge the financial support for
260 this study from the Malaysian Ministry of Higher Education
261 (MOHE) through the Fundamental Research Grant Scheme
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